Journal of the American Chemical Society
Time-Resolved Formation and Operation Maps of Pd Catalysts Suggest a Key Role of Single Atom Centers in Cross-Coupling
Publication type: Journal Article
Publication date: 2023-04-13
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor: 15
ISSN: 00027863, 15205126
General Chemistry
Catalysis
Biochemistry
Colloid and Surface Chemistry
Abstract
An approach to the spatially localized characterization of supported catalysts over a reaction course is proposed. It consists of a combination of scanning, transmission, and high-resolution scanning transmission electron microscopy to determine metal particles from arrays of surface nanoparticles to individual nanoparticles and individual atoms. The study of the evolution of specific metal catalyst particles at different scale levels over time, particularly before and after the cross-coupling catalytic reaction, made it possible to approach the concept of 4D catalysis–tracking the positions of catalytic centers in space (3D) over time (+1D). The dynamic behavior of individual palladium atoms and nanoparticles in cross-coupling reactions was recorded with nanometer accuracy via the precise localization of catalytic centers. Single atoms of palladium leach out into solution from the support under the action of the catalytic system, where they exhibit extremely high catalytic activity compared to surface metal nanoparticles. Monoatomic centers, which make up only approximately 1% of palladium in the Pd/C system, provide more than 99% of the catalytic activity. The remaining palladium nanoparticles changed their shape and could move over the surface of the support, which was recorded by processing images of the array of nanoparticles with a neural network and aligning them using automatically detected keypoints. The study reveals a novel opportunity for single-atom catalysis─easier detachment (capture) from (on) the carbon support surface is the origin of superior catalytic activity, rather than the operation of single atomic catalytic centers on the surface of the support, as is typically assumed.
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- We do not take into account publications that without a DOI.
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- Statistics recalculated weekly.
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Galushko A. S. et al. Time-Resolved Formation and Operation Maps of Pd Catalysts Suggest a Key Role of Single Atom Centers in Cross-Coupling // Journal of the American Chemical Society. 2023.
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Galushko A. S., Boiko D. A., Pentsak E. O., Eremin D. B., Ananikov V. P. Time-Resolved Formation and Operation Maps of Pd Catalysts Suggest a Key Role of Single Atom Centers in Cross-Coupling // Journal of the American Chemical Society. 2023.
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TY - JOUR
DO - 10.1021/jacs.3c00645
UR - https://doi.org/10.1021%2Fjacs.3c00645
TI - Time-Resolved Formation and Operation Maps of Pd Catalysts Suggest a Key Role of Single Atom Centers in Cross-Coupling
T2 - Journal of the American Chemical Society
AU - Galushko, Alexey S
AU - Boiko, Daniil A.
AU - Pentsak, Evgeniy O
AU - Eremin, Dmitry B.
AU - Ananikov, Valentine P.
PY - 2023
DA - 2023/04/13 00:00:00
PB - American Chemical Society (ACS)
SN - 0002-7863
SN - 1520-5126
ER -
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@article{2023_Galushko,
author = {Alexey S Galushko and Daniil A. Boiko and Evgeniy O Pentsak and Dmitry B. Eremin and Valentine P. Ananikov},
title = {Time-Resolved Formation and Operation Maps of Pd Catalysts Suggest a Key Role of Single Atom Centers in Cross-Coupling},
journal = {Journal of the American Chemical Society},
year = {2023},
publisher = {American Chemical Society (ACS)},
month = {apr},
url = {https://doi.org/10.1021%2Fjacs.3c00645},
doi = {10.1021/jacs.3c00645}
}